KR940011170B1 - Polyarylene sulfide resin composition - Google Patents

Abstract

A polyarylene sulphide composition having improved mechanical properties and excellent surface appearance when molded comprises (A) 99 to 20 parts by weight of polyarylene sulphide, (B) 1 to 80 parts by weight of a polyamide and (C) 0.01 to 5 parts by weight, based on 100 parts by weight of (A) and (B) in total, of an alkoxysilane. It may further comprise (D) up to 400 parts by weight of a filler in the form of fiber, particles or plates. It can be produced by blending (A), (B) (C) and (D) with one another and melt-kneading the blend for at least 30 seconds while heated.

Description

Polyarylene Sulfide Resin Composition

The present invention is directed to an improved polyarylene sulfide resin composition and a method for preparing the same. Specifically, the present invention relates to a polyarylene sulfide resin composition having improved impact resistance and ductility, and excellent appearance on the surface of a molded article, and a method for producing the same.

In recent years, flame-retardant thermoplastic resins having high heat resistance and chemical resistance have been demanded as components for electric and product components and parts for automobiles and chemical devices. Polyarylene sulfide resins represented by polysulfide phenylene resins are one of the resins that meet these demands, and since they have good properties in terms of cost, the demand for them is increasing. However, this resin has a serious drawback that is low in ductility and brittle. It is known that properties such as strength, hardness, toughness and heat resistance required for engineering plastics can be significantly improved by incorporating fibrous reinforcing materials such as glass fibers or carbon fibers into the resin.

However, incorporation of fibrous reinforcements into resins is more fragile than other engineering plastics such as nylon or polyacetal. Therefore, the use of this resin for various purposes is limited because the toughness is insufficient despite having excellent properties.

To solve this problem, the following methods have been proposed. (1) A method of mixing up to 10% by weight of unsaturated carboxylic acid or anhydride thereof, graft-copolymerized α-olefin copolymer and epoxy resin (see Japanese Patent Laid-Open No. 207921/1984), (2 ) a method of incorporating an olefin copolymer comprising an α-olefin and a glycidyl ester of an αβ-unsaturated acid (see Japanese Patent Laid-Open No. 189166/1984), and (3) a method of incorporating a polyamide resin and an epoxy resin. (See Japanese Patent Laid-Open No. 155462/1984).

However, these methods are still insufficient because each still suffers from problems.

In the above methods (1) and (2), the polyarylene sulfide resin is combined with an olefin copolymer having an ester bond to improve the toughness. However, according to the following tests of the present inventors, since the molding temperature of the polyarylene sulfide resin is about 300 to 320 ° C., the olefin copolymer is decomposed in the molding step, so that the toughness of the molded article is insufficient.

According to this test, the method (3) is practically unsatisfactory because the flow is observed at the surface of the molded article and the surface condition is poor, so that the melt flow stability of the composition is very low.

The polyarylene sulfide composition is composed of (A) 99 to 20 parts by weight of polyarylene sulfide, (B) 1 to 80 parts by weight of polyamide and (C) 100 alkoxysilanes based on 100 parts by weight of (A) and (B). It consists of 0.01-5 weight part. (D) up to 400 parts by weight of the filler may be further included in the form of fibers, particles or plates. It can be prepared by combining (A), (B), (C) and (D) with other components and melting-kneading the formulation for at least 30 seconds while heating.

The composition of the present invention comprises two implementations. Implementation (1) is based on (A) 97 to 20 parts by weight of polyarylene sulfide, (B) 3 to 80 parts by weight of polyamide and (C) 100 parts by weight of total (A) and (B), and alkoxysilane And 0.01 to 5 parts by weight of an alkoxysilane selected from the group consisting of an epoxy alcohol silane, an aminoalkoxysilane and a mercaptoalkoxysilane.

Implementation (2) comprises (A) 99 to 20 parts by weight of polyarylene sulfide, (B) 1 to 80 parts by weight of polyamide elastomer, (B ') up to 79 parts by weight of polyamide and (C) total (A) And 0.01 to 5 parts by weight of alkoxysilane based on 100 parts by weight of (B) and (B '). The alkoxysilane of the embodiment (2) is preferably selected from vinylalkoxysilane, epoxyalkoxysilane, aminoalkoxysilane, mercaptoalkoxysilane and arylalkoxysilane.

The present invention will be described below with reference to these two implementations. As a result of intensive research for the purpose of improving the toughness of the polyarylene sulfide resin composition and the appearance of the molded article surface, the present inventors have found the reactive end of the high toughness arylene sulfide and polyamide resin. The present inventors further studied for the purpose of finding a reactant in which both resins react with both of the resins under the condition that the main chain of the resin is not cleaved. As a result, the present inventors, when kneading a silane compound having an alkoxyl group in the molecule with polyarylene sulfide and polyamide resin at a specific temperature for a certain time, can produce a molded article having a significantly high toughness and a beautiful surface. It has been found that molding materials that can be used can be made. The present invention has been completed based on this finding.

Therefore, the present invention provides a polyarylene sulfide resin composition, comprising 100 parts by weight of the total resin component as follows. : Selected from the group consisting of (A) 97 to 20 parts by weight of polyarylene sulfide resin, (B) 3 to 80 parts by weight of polyamide resin, (C) alkoxysilane, epoxyalkoxysilane, aminoalkoxysilane and mercaptoalkoxysilane 0.01 to 5 parts by weight of at least one silin compound, and (D) 0 to 400 parts by weight of a filler selected from fibrous fillers, particulate fillers and plate fillers or mixtures thereof.

And the process for producing the polyarylene sulfide resin composition is characterized by melt-kneading together (A), (B) and (C) and, if necessary, component (D) under heating for at least 30 seconds.

The polyarylene sulfide resin used in the composition of the present invention (A) is mainly a repeating unit Wherein Ar represents an arylene group.

Arylene group Silver p-phenylene group m-phenylene group o-phenylene group Substituted phenylene groups

Provided that R represents an alkyl group, preferably a C ₁ to C ₅ alkyl group or a phenyl group, Is an integer from 1 to 4.

p, p'-diphenylene sulfone group p, p'-biphenylene group p, p'-diphenylene ether group p, p'-diphenylenecarbonyl group Naphthalene group It includes.

A polymer composed of only one type of repeating unit selected from the arylene sulfide group having the arylene group, i.e., a homopolymer may be used. In view of processability of the composition, a copolymer composed of two or more repeating units may be preferable.

As a homopolymer, the substantially linear copolymer which consists of a sulfide p-phenylene group whose arylene group is a p-phenylene group as a repeating unit is especially preferable.

In order to form a copolymer, a combination of two or more arylene sulfides composed of the arylene group may be used. Among these, the combination which consists of sulfide m-phenylene group and sulfide p-phenylene group is especially preferable. Of these, for example, substantially linear copolymers containing at least 50 mol%, preferably at least 60 mol%, more preferably 70 mol% of sulfided p-phenylene groups are suitable in view of heat resistance, moldability and mechanical properties. The amount of sulfide m-phenylene group is 5 to 50 mol%, preferably 10 to 25 mol%.

In the arrangement of the repeating unit, the block arrangement (for example, described in Japanese Patent Laid-Open No. 1428/1986) is better than the random arrangement in terms of heat resistance and mechanical properties, and workability in both cases is excellent. It is almost equivalent but it is preferable to use block arrangement.

In the present invention, as the polyarylene sulfide resin used as the component (A), a polymer having increased melt viscosity and improved moldability, which is prepared by curing by oxidative crosslinking and thermal crosslinking of the polymer, can be used. Moreover, the substantially linear structure obtained by multicondensing the monomer which consists mainly of a bifunctional monomer can be used. The properties of molded articles made of later polymers having a substantially linear structure are usually superior to those made of the preceding polymers.

As the polyarylene sulfide resin of the present invention, the molded polymer is mixed with a crosslinked arylene sulfide resin prepared by polymerizing a monomer having a gel state when melting and having three or more functional groups with another monomer. It is preferable to further use the mixed resin produced by the above polymer.

Examples of the polyamide resin (B) used in the present invention include dicarboxylic acids such as dicarboxylic acid oxalic acid, adipic acid, suberic acid, sebacic acid, terephthalic acid, isophthalic acid or 1,4-cyclohexyldicarboxylic acid. Various known compounds such as, for example, polyamide resins prepared by polycondensation with diamines such as ethylenediamine, pentamethylenediamine, hexamethylenediamine, decamethylenediamine, 1,4-cyclohexyldiamine or m-xylylenediamine There are things; Polyamide resins are prepared, for example, by polymerizing cyclic lactams, such as caprolactam or laurolactam, or by copolymerizing cyclic lactams with salts of dicarboxylic acids and diamines. Among these polyamide resins, nylon 6, nylon 66, nylon 6, 10, nylon 66/6, 10, nylon 6/66, nylon 12 and the like are preferable. Of these, nylon 6 and nylon 66 are preferred. The polyamide resin to be used is preferably moisture content below a predetermined limit, and therefore preferably dried before use.

The amount of the polyamide resin (B) used in the present invention is preferably 3 to 80% by weight, with the total weight of the components (A) and (B) as the molar. When the amount of component (B) is insufficient, the toughness is unsatisfactory, and when exceeded, the advantages of the polyarylene sulfide resin (A) are damaged.

Component (C) which can be used in the present invention includes vinylalkoxysilane, epoxyalkoxysilane, aminoalkoxysilane and mercaptoalkoxysilane. These may be used alone or in combination of two or more. Examples of the vinylalkoxysilanes include vinyltriethoxysilane, vinyltrimethoxysilane, and vinyl tris (β-methoxyethoxy) silane.

Examples of the epoxyalkoxysilanes include gamma-glycidoxy propyl trimethoxysilane and gamma-glycidoxy propyl triethoxysilane.

Examples of aminoalkoxysilanes include γ-amino-propyltrimethoxysilane, γ-amino-propyltriethoxysilane, γ-aminopropylmethyldimethoxysilane, γ-aminopropylmethyldiethoxysilane and N- (β-aminoethyl) -γ-aminopropyltriethoxysilane and N-phenyl-γ-aminopropyltrimethoxysilane.

As mercaptoalkoxysilanes, there are γ-mercaptopropyltrimethoxysilane and γ-mercaptopropyltriethoxysilane.

The amount of the alkoxysilane compound used as component (C) is from 0.01 to 5 parts by weight, preferably based on 100 parts by weight of the total weight of polyarylene sulfide resin [component (A)] and polyamide resin [component (B)]. 0.5 to 3 parts by weight.

The amount of alkoxysilane compound added varies depending on the kind of compound and the use of the composition. If the amount is insufficient, the effect of improving the toughness is insufficient, while if the amount is exceeded, the melt viscosity is excessively increased to excite defects in the molding operation.

The fillers used as component (D) are not always indispensable, but they are preferably used to produce molded articles having excellent properties such as, for example, mechanical strength, heat resistance, dimensional stability and electrical properties. Depending on the application, fibrous, particulate, or plate fillers are used.

Fibrous fillers include, for example, inorganic fibrous materials such as fibers of glass, asbestos, carbon, silica, silica / alumina, zirconia, boron nitride, silicon nitride, boron titanate and sodium titanate, and fibers such as stainless steel, aluminum, titanium, grit and brass There is a metal fiber such as. Among these, typical fibrous fillers are glass fibers and carbon fibers. It is also possible to use high-melting organic fibrous materials such as, for example, polyamides, fluororesins and acrylic resins.

Particulate fillers include carbon black, silica, quartz powders, glass beads, glass powders such as calcium silicates, aluminum silicates, kaolin talc, silicates such as clay, diatomaceous earth and wollastonite, for example metal oxides such as iron oxide, titanium oxide and alumina, for example Metal carbonates such as calcium carbonate and magnesium carbonate, such as metal sulfates such as calcium sulfate and barium sulfate, silicon carbide, silicon nitride, boron nitride and various metal powders.

Plate-like fillers include mica, glass flakes and various metal foils. These inorganic fillers may be used alone or in combination of two or more thereof. The combination of fibrous fillers, in particular glass fibers or carbon fibers with particulate fibers or plate fibers, is particularly preferred for obtaining good mechanical strength, dimensional accuracy and electrical properties.

The composition of the present invention can be prepared by various known methods. However, it is essential to knead at least three components (A) (B) and (C) together for at least 30 seconds in a molten state. In particular components (A), (B) and (C) and, if necessary, components (D) and other components, before the mixture is fed to a single-screw or double-blade screw extruder and melt drilled to form pellets Mix homogeneously with a mixer such as a tumbler mixer or a Henschel mixer. In this step, some or all of the components (A) and (B) are crushed and first a part of the resin is mixed homogeneously with the component (C) in the blender, then the resulting mixture is further mixed with the rest and melted. Component (D) may be added during or after the melting step.

The treatment temperature is preferably 5 to 100 ° C., particularly 10 to 60 ° C. higher than the melting point of the resin component. Too high a temperature undesirably leads to decomposition and abnormal reactions.

Depending on the treatment temperature and the type and amount of the silane compound, various treatment times range from 30 seconds to 15 minutes, with 1 to 10 minutes being preferred.

Although the detailed mechanism of the effect of the alkoxysilane compound of the present invention is not yet fully understood, the polyarylene sulfide molecule is bound to the polyamide molecule by the silane compound to mutually improve the compatibility of components (A) and (B). I guess it is. This mechanism was confirmed by electron microscope observation of the cross section of the molded article manufactured from the composition of the present invention.

The compositions of the present invention may contain antioxidants, heat stabilizers, lubricants, nucleating agents, ultraviolet absorbers, colorants, demolders and other general auxiliaries within the object of the present invention. Such adjuvants may be incorporated into the resin composition during the melt-kneading treatment or at any other stage.

The polyarylene sulfide resin composition of the present invention has the following effects: (1) Molded articles made of the present invention have improved mechanical properties such as tensile elongation and impact resistance, and (2) mechanical properties It is well balanced, (3) the appearance of the molded article is beautiful, and (4) the auxiliary agent is inexpensive, so that the resin composition can be produced at low cost and easily extruded and kneaded.

A second embodiment of the present invention provides a polyarylene sulfide composition comprising 100 parts by weight of the following total resin composition. (A) 99 to 20 parts by weight of polyarylene sulfide resin, (B) 1 to 80 parts by weight of polyamide elastomeric resin, and (B ') 0 to 79 parts by weight of polyamide resin, and (C) 0.01 to 5 Parts by weight of alkoxysilane and

(D) 0 to 400 parts by weight of a filler consisting of fibrous fillers, particulate fillers and plate fillers or mixtures thereof.

In addition, the method for preparing the polyarylene sulfide resin composition comprises the components (A), (B) and (C), and if necessary, the components (B ') and (D) melt together for at least 30 seconds under heating. -Has the characteristics to be kneaded.

The polyarylene sulfide resin used as component (A) of the composition of the present invention is mainly a repeating unit Wherein Ar represents an arylene group.

In the present invention, the polyamide elastomer resin used as component (B) is a block copolymer composed of a hard piece of polyamide and a soft piece having a Young's modulus (23 ° C., 50% relative humidity) of less than 10,000 kgf / cm 2. to be.

Typical examples of soft elastomeric pieces are polyalkylene oxides, in particular those having a molecular weight of 400 to 60,000 and having 2 to 6 carbon atoms in the alkylene group.

Various methods have been reported for the synthesis of such polyamide elastomers. Generally, a method comprising two steps, namely, forming a nylon oligomer and polymerizing by esterification is used.

Polyamide components that can be used as solid pieces herein include polyamide 6, polyamide 66, polyamide 6, 12, polyamide 11 and polyamide 12.

Polyether components that can be used in the soft flakes herein are polyoxyethylene glycol, polyoxypropylene glycol and polyoxytetramethylene glycol.

The polyamide elastomeric resin (B) used preferably has a water content below a predetermined limit and is preferably dried before use.

The amount of polyamide elastomer resin (B) used varies depending on the application. This amount is preferably 1 to 88 parts by weight based on 99 to 20 parts by weight of polyarylene sulfide resin. Furthermore, the amount of 5 to 80 parts by weight relative to 95 to 20 parts by weight of polyarylene sulfide resin is more preferable. If this amount is less than 1 weight part, the toughness improvement effect of a resin composition will not appear at all.

Although polyamide resin (B ') is indispensable in this invention, it can also be used in combination with polyamide elastic-polymer resin (B).

Polyamide resin (B ') is a polyamide having a Young's modulus of warpage of at least 10,000 kgf / cm 2 (23 ° C., 50% relative humidity). It has a high affinity for polyamide elastomers, controls the mechanical properties, in particular the elasticity of the composition as a whole, and is less expensive than polyamide elastomer resins. Therefore, it is preferable to be used for producing a molded article having excellent mechanical strength and heat resistance at low cost. However, using too much amount is undesirable because it impairs wettability.

The polyamide resin (B ') is the polyamide (B) of the first embodiment. The present invention is characterized in that an alkoxysilane compound (C) is used in combination with the resin composition.

Alkoxysilanes (C) that can be used in the present invention include vinylalkoxysilanes, epoxyalkoxysilanes, aminoalkoxysilanes, mercaptoalkoxysilanes and arylalkoxysilanes.

These may be used alone or in combination of two or more.

Vinylalkoxysilanes include vinyltriethoxysilane, vinyltrimethoxysilane and vinyltris (β-methoxyethoxy) silane.

Examples of the epoxyalkoxysilanes include γ-glycidoxypropyltrimethoxysilane, β- (3,4-epoxycyclohexyl) -ethyltrimethoxysilane, and γ-glycidoxypropyltriethoxysilane.

Examples of aminoalkoxysilanes include γ-aminopropyltrimethoxysilane, γ-aminopropyltriethoxysilane, γ-aminopropylmethyldimethoxysilane, γ-aminopropylmethyldiethoxysilane, and N-phenyl-γ-aminopropyltrimeth Oxysilanes.

As mercaptoalkoxysilane, (gamma)-mercaptopropyl trimethoxysilane and (gamma)-mercaptopropyl triethoxysilane.

Examples of allyl alkoxysilanes include gamma -diallylaminopropyltrimethoxysilane, gamma -allylaminopropyltrimethoxysilane and gamma -allylthiopropyltrimethoxysilane.

The amount of the alkoxysilane compound used as component (C) is 100 of the total of polyarylene sulfide resin [component (A)], polyamide elastomer resin [component (B)] and polyamide resin [component (B ')]. 0.01 to 5 parts by weight, preferably 0.1 to 3 parts by weight, based on parts by weight.

The amount of alkoxysilane compound added varies depending on the kind of compound and the use of the composition. If this amount is insufficient, the effect of improving the toughness is insufficient, whereas if it is exceeded, the melt viscosity is excessively increased to cause a defect in the molding operation.

The amount of the inorganic filler is 400 parts or less based on 100 parts by weight of the total of the resin components (A), (B) and (C). If the amount exceeds 400 parts by weight, formability and toughness are undesirably impaired. This amount is particularly preferably less than 250 parts by weight.

The composition of the present invention can be prepared by various known methods. However, it is essential to knead at least three components (A), (B) and (C) and, if necessary, component (B ') together in a molten state for at least 30 seconds.

In particular, for example components (A), (B), (C) and (B ') and, if necessary, components (D) and other components, the mixture is fed to a single-screw or double-blade-screw extruder to pellet Mix homogeneously using a mixer, such as a tumbler or a Henschel mixer, prior to forming. In this step, part or all of the components (A), (B) and (B ') are crushed and firstly a part of the resin is uniformly mixed with component (C) in the blender, and then the resulting mixture is further mixed with the rest. Mix and melt.

Component (D) can be added during or after the melting step.

Component (D) is preferably added after the polymer component is melt-kneaded and reacted with component (C) in order to obtain a significant toughness improving effect.

The treatment temperature is preferably 5 to 100 ° C., particularly 10 to 60 ° C. higher than the melting point of the resin component. Too high a temperature undesirably leads to decomposition and abnormal reactions.

The melt treatment time varies depending on the treatment temperature and the type and amount of the silane compound, and the treatment time is in the range of 30 seconds to 15 minutes, preferably 1 to 10 minutes.

Although the detailed mechanism of the effect of the alkoxysilane compound of the present invention is not yet fully understood, the polyarylene sulfide molecule is bound to the polyamide molecule by the silane compound to form components (A), (B) and (B '). It is speculated to improve mutual compatibility. This mechanism was confirmed by observing the fact that the viscosity increases with the melt treatment carried out in the presence of component (C), and also by observing the cross-sectional structure of the molded article produced according to the present invention. According to the method of the present invention, the polyamide resin may be dispersed in the form of fine particles (1 μm or more), but in the absence of the silane compound (C), it is dispersed in the form of very large particles (10 μm or more).

From the above description and the following examples, it will be apparent that the resin composition of the present invention is very finely dispersed in the polyarylene sulfide resin composition of the present invention and the composition of the present invention has the following effects.

(1) Molded articles made of the composition of the present invention have significantly improved mechanical properties such as, for example, tensile elongation and impact resistance,

(2) mechanical properties are well balanced with heat resistance,

(3) The appearance of the molded article is beautiful.

Example 1

The following examples are intended to illustrate the invention in more detail and are not intended to limit the invention in any way.

[Examples 1 to 5 and Comparative Examples 1 and 2]

40 parts by weight of nylon 66 were added to 60 parts by weight of polyphenylene sulfide polymer (m.p. 285 ° C., melt viscosity measured at shear rate of 1200 / sec at 310 ° C .: about 500 P).

Here, γ-aminopropyltriethoxysilane and, as necessary, glass fibers (cutting yarns having a diameter of 10 μm and a length of 3 mm) were added in the amounts specified in Table 1.

These were premixed for 5 minutes on a Henschel mixer.

The mixture was melt-kneaded with an extruder having a cylinder temperature of 310 ° C. to prepare pellets of a polysulfide phenylene resin composition.

The pellets were then made into SATM test pieces with an injection molding machine having a cylinder temperature of 310 ° C. and a molding temperature of 150 ° C.

This specimen was subjected to tensile, impact and thermal deformation tests.

The appearance of the molded article surface was visually evaluated.

The results are summarized in Table 1.

[Examples 6 to 9 Comparative Examples 3 and 4]

Nylon 66 was added to the same polysulfide phenylene as used in the Examples and Comparative Examples in the ratios shown in Table 2.

To this, γ-aminopropyltriethoxysilane and glass fibers were added in the ratios shown in Table 2 and the same steps as in Examples 1 to 5 were repeated.

The results are shown in Table 2.

[Examples 10 and 11 and Comparative Examples 5 and 6]

40 parts by weight of nylon 6 was added to 60 parts by weight of the same polysulfide phenylene polymer. Then, aminopropyltriethoxysilane and glass fibers were added thereto in the amounts specified in Table 3.

Then, the same process as in Examples 1 to 5 was repeated.

The results are shown in Table 3.

[Examples 12 and 13 and Comparative Examples 7 and 8]

40 parts by weight of nylon 12 was added to 60 parts by weight of the same polysulfide phenylene polymer as used in the above examples.

Then γ-aminopropyltriethoxysilane and glass fibers were added thereto in the amounts specified in Table 4.

The same process as in Examples 4 to 5 was repeated.

The results are shown in Table 4.

EXAMPLE 14 AND 15

40 parts by weight of nylon 66 was added to 60 parts by weight of the same polysulfide phenylene polymer as used in the above examples.

Next, gamma-glycidoxy propyl trimethoxysilane and glass fibers were added thereto in the amounts specified in Table 5.

The same process as in Examples 1 to 5 was repeated.

The results are shown in Table 5 together with the results of Comparative Examples 1 and 2.

[Examples 16 and 17]

The same process as in Examples 14 and 15 was repeated except that γ- glycidoxypropyltrimethoxysilane was replaced with γ-merrabtopropyltrimethoxysilane in the amounts specified in Table 6.

The results are shown in Table 6 together with the results of Comparative Examples 1 and 2.

[Examples 18 and 19]

The same process as in Examples 14 and 15 was repeated, but the γ- glycidoxypropyltrimethoxysilane was replaced with the amount of vinyl trimethoxysilane in the amounts specified in Table 7.

The results are shown in Table 7 together with the results of Comparative Examples 1 and 2.

TABLE 1

TABLE 2

TABLE 3

TABLE 4

TABLE 5

TABLE 6

TABLE 7

[Examples 19 and 23 and Comparative Examples 3 and 4]

20 parts by weight of polyamide elastomer (trade name: Daiamid E 62, Daicel-Huls Corporation ^* ) (see Note 1 below) was added to 80 parts by weight of polysulfide phenylene polymer (mp 285 ° C.). To this was added γ-aminopropylethoxysilane and, as necessary, glass fibers (cut yarns having a diameter of 10 μm and a length of 3 mm) in the amounts specified in Table 8. The mixture was melt-kneaded with an extruder having a cylinder temperature of 310 ° C. to prepare pellets of the polysulfide phenylene resin composition.

The pellets were then made into ASTM test pieces using an injection molding machine having a cylinder temperature of 310 ° C. and a molding temperature of 150 ° C.

This test piece was tested for tensile, impact and heat resistance.

The appearance of the molded article surface was visually evaluated.

The results are summarized in Table 8.

^* 1 Polyamide elastomer consisting of nylon 12 as a hard piece and polybutylene as a soft piece (bending Young's modulus: 3500 kg / c / m 2)

[Examples 24 to 27 and Comparative Examples 5 and 6]

Daiamid E 62 was added to the same polysulfidephenylene polymers used in the examples and comparative examples in the proportions indicated in Table 9.

To this was added γ-aminopropyl triethoxysilane and glass fibers in the proportions indicated in Table 9, and the same steps as in Examples 19 to 23 were repeated.

The results are shown in Table 9.

[Examples 28 to 35]

20 parts by weight of polyamide elastomer (Daiamid E62) was added to the same 80 parts by weight of polysulfide phenylene.

Then γ-glycidoxypropyltrimethoxysilane, γ-mercaptopropyl trimethoxysilane, vinyltrimethoxysilane or γ-diallylaminopropyltrimethoxysilane and glass fibers are listed here. Add by amount.

The same process as in Examples 19 to 23 was repeated.

The results are shown in Table 10.

[Examples 36 to 40 and Comparative Examples 7 and 8]

To 60 parts by weight of the same polysulfide phenylene polymer was added polyamide elastomer (Daiamid E 62) and polyamide (PA) 66 in the amounts specified in Table 11.

2 parts by weight of gamma -aminopropyltriethoxysilane and, as necessary, glass fibers were added to 100 parts by weight of the total mixture obtained as described above.

Then the same process as in Examples 19 to 23 was repeated.

The results are shown in Table 11.

[Examples 41 to 50 and Comparative Examples 9 and 10]

The poly-phenylene sulfide polymer of 20 wt parts of the polyamide elastomer of 80 wt%: a (trade name Daiamid E 40, Daicel-Huls main product ^*) (see Note 2 below) was added.

Then γ-aminopropyltriethoxysilane, γ-glycidoxypropyltrimethoxysilane, γ-mercaptopropyltrimethoxysilane, vinyltrimethoxysilane or γ-diallylaminopropyltrimethoxy Silane and, as necessary, glass fibers were added in the amounts specified in Table 12.

Then, the same process as in Examples 19 to 23 was repeated.

The results are shown in Table 12.

(Note 2) ^* Polyamide elastomer composed of nylon 12 as a hard piece and polyoxybutylene as a soft piece (bending Young's modulus: 900 kgf / cm 2)

TABLE 8

TABLE 9

TABLE 10

TABLE 11

TABLE 12

Claims (4)

(A) 99 to 20 parts by weight of polyarylene sulfide, (B) 1 to 80 parts by weight of polyamide, and (C) basically 0.01 to 5 parts by weight of alkoxysilane with 100 parts by weight of the sum of (A) and (B) Polyarylene sulfide composition which consists of parts. The composition according to claim 1, further comprising (D) 400 parts by weight or less of fiber, particles, or plate-shaped fillers. The method of claim 1 or 2, wherein (A) 97 to 20 parts by weight of polyarylene sulfide, (B) 3 to 80 parts by weight of polyamide, and (C) basically the sum of (A) and (B) is 100 A composition comprising 0.01 to 5 parts by weight of an alkoxysilane selected from the group consisting of alkoxysilanes, epoxysilanes, aminoalkoxysilanes and mercaptoalkoxysilanes. In order to prepare the composition of claim 1, the steps of mixing (A), (B), (C) and (D) with another component and heating the mixture for at least 30 seconds-melt kneading Characterized in that the method.